Glycine for Enhanced Water Imbibition in Carbonate Reservoirs – What is the Role of Amino Group?

I. Baghishov, Gayan A. Abeykoon, Mingyuan Wang, Francisco J. Argüelles Vivas, R. Okuno
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引用次数: 1

Abstract

Previous studies indicated the efficacy of the simplest amino acid, glycine, as an aqueous additive for enhanced water imbibition in carbonate reservoirs. The objective of this research was to investigate the importance of the amino group of glycine in its enhanced water imbibition. To this end, glycine was compared with two carboxylates (acetate and formate) with/without adding hydrogen chloride (HCl) for adjusting the solution pH. Note that the amino group is the only difference between glycine and acetate. Contact-angle experiments on calcite were carried out at 347 K and atmospheric pressure with 68000-ppm reservoir brine (RB), and 4 different concentrations of glycine, acetate, and formate solutions in RB. To test the hypothesis that calcite dissolution is one of the main mechanisms in wettability alteration by glycine, we performed another set of contact angle experiments by adding HCl to brine, acetate, and formate solutions. HCl was added to match the pH of the glycine solution at the same concentration. We also performed imbibition tests with Texas Cream Limestone cores at 347 K with brine, glycine, acetate, and formate solutions (with and without HCl) in RB at 5.0 wt%. Contact-angle results indicated that glycine changed calcite's wettability from oil-wet to water-wet (45°). However, acetate solution was not able to change the wettability to water-wet; and formate moderately decreased the contact angle to 80°. The pH level increased from 6.1 to 7.6 after the contact angle experiment in glycine solution, indicating the consumption of hydrogen ions due to calcite dissolution. The levels of pH in formate and acetate solutions, however, decreased from 8.4 to 7.8. The acidity of glycine above its isoelectric point arises from the deprotonation of the carboxyl group. Imbibition tests with carbonate cores supported the observations from the contact-angle experiments. The oil recovery was 31% for glycine solution, 20% for RB, 21% for formate solution, and 19% for acetate solution. This re-confirmed the effectiveness of glycine as an additive to improve the oil recovery from carbonates. An additional set of imbibition tests revealed that acetate at the pH reduced to the same level as glycine was still not able to recover as much oil as glycine. This showed that glycine recovered oil not only because of the calcite dissolution and the carboxyl group, but also because of the amino group. It is hypothesized that the amino group with its electron donor ability creates a chelation effect that makes glycine entropically more favorable to get attached to the calcite surface than acetate. Another important result is that the formate solution at an adjusted pH resulted in a greater oil recovery than RB or RB at the same pH. This indicates that there is an optimal pH for the carboxyl group to be effective in wettability alteration as also indicated by the pH change during the contact-angle experiment.
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甘氨酸在碳酸盐储层中增强吸水性——氨基的作用是什么?
先前的研究表明,最简单的氨基酸甘氨酸作为一种水性添加剂,可以增强碳酸盐岩储层的吸水性。本研究的目的是探讨氨基甘氨酸在其增强吸水性中的重要性。为此,甘氨酸与两种羧酸盐(乙酸酯和甲酸酯)在加入/不加入氯化氢(HCl)的情况下进行了比较,以调整溶液的ph。注意,氨基是甘氨酸和乙酸酯之间唯一的区别。在347 K和常压条件下,用68000-ppm的储层盐水(RB)和4种不同浓度的甘氨酸、乙酸盐和甲酸盐溶液对方解石进行了接触角实验。为了验证方解石溶解是甘氨酸改变润湿性的主要机制之一的假设,我们通过在盐水、醋酸盐和甲酸盐溶液中加入HCl进行了另一组接触角实验。在相同浓度下,加入与甘氨酸溶液pH相匹配的盐酸。我们还对德克萨斯奶油石灰石岩心进行了渗吸测试,温度为347 K,在5.0 wt%的RB中加入盐水、甘氨酸、乙酸盐和甲酸盐溶液(含或不含HCl)。接触角结果表明,甘氨酸使方解石的润湿性由亲油型变为亲水型(45°)。然而,醋酸溶液不能改变润湿性为水湿性;甲酸盐适度降低接触角至80°。甘氨酸溶液中接触角实验结束后pH值由6.1上升到7.6,说明方解石溶解导致氢离子消耗。甲酸盐和醋酸盐溶液的pH值则从8.4降至7.8。甘氨酸在其等电点以上的酸度是由羧基的去质子化引起的。碳酸盐岩心渗吸实验支持了接触角实验的结果。甘氨酸溶液的采收率为31%,RB溶液为20%,甲酸溶液为21%,乙酸溶液为19%。这再次证实了甘氨酸作为添加剂在提高碳酸盐原油采收率方面的有效性。另一组吸胀试验表明,当pH值降低到与甘氨酸相同的水平时,乙酸盐仍然不能像甘氨酸那样回收那么多的油。这表明甘氨酸回收油不仅是因为方解石的溶解和羧基,还因为氨基。假设具有电子供体能力的氨基产生螯合效应,使甘氨酸在熵上比醋酸盐更有利于附着在方解石表面。另一个重要的结果是,调整pH后的甲酸溶液比相同pH下的RB或RB的采收率更高。这表明羧基有效改变润湿性存在一个最佳pH值,接触角实验中pH的变化也表明了这一点。
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